Rational Molecular Design Enables Efficient Blue TADF-OLEDs with Flexible Graphene Substrate

Observation of thermally activated delayed fluorescence (TADF) in conjugated systems redefined the molecular design approach to realize highly efficient organic light emitting diodes (OLEDs) in the early 2010s. Enabling effective reverse intersystem crossing (RISC) by minimizing the difference between singlet and triplet excited state energies (Delta E-ST) is proven to be a widely applicable and fruitful approach, which results in remarkable external quantum efficiencies (EQE). The efficacy of RISC in these systems is mainly dictated by the first-order mixing coefficient (lambda), which is proportional to spin-orbit coupling (H-SO) and inversely proportional to Delta E-ST. While minimizing Delta E-ST has been the focus of the OLED community over the last decade, the effect of H-SO in these systems is largely overlooked. Here, molecular systems with increased H-SO are designed and synthesized by substituting selected heteroatoms of high-performance TADF materials with heavy-atom selenium. A new series of multicolor TADF materials with remarkable EQEs are achieved. One of these materials, SeDF-B, results in pure blue emission with EQEs approaching 20%. Additionally, flexible graphene-based electrodes are developed for OLEDs and revealed to have similar performance as standard indium tin oxide (ITO) in most cases. These devices are the first report of TADF based OLEDs that utilize graphene-based anodes.

Automated summary

Observation of thermally activated delayed fluorescence (TADF) has revolutionized the molecular design of highly efficient OLEDs. The effectiveness of TADF is largely determined by the first-order mixing coefficient (lambda) and the difference between singlet and triplet excited state energies (Delta E-ST). While Delta E-ST has been the main focus, the influence of spin-orbit coupling (H-SO) has been overlooked. In this study, TADF materials with increased H-SO are achieved by substituting heteroatoms with heavy-atom selenium, resulting in remarkable EQEs.